Precisely constructing orbital coupling-modulated iron dinuclear site for enhanced catalytic ozonation performance

Area of Science:

• Heterogeneous Catalysis
• Materials Science
• Environmental Chemistry

Background:

• Atomically precise dinuclear heterogeneous catalysts offer potential for efficient catalytic ozonation.
• Understanding synergy mechanisms in catalytic reactions is crucial for performance enhancement.

Purpose of the Study:

• To construct and investigate Fe2 dinuclear sites for catalytic ozonation.
• To elucidate the structure-activity relationship at the atomic level.

Main Methods:

• A "ship-in-a-bottle and pyrolysis" strategy using Fe2(CO)9 dinuclear-cluster.
• Systematic characterizations and theoretical modeling.
• Testing catalytic ozonation efficiency for CH3SH elimination.

Main Results:

• Precisely constructed Fe2 sites with Fe-Fe bonds on N-doped carbon.
• Fe-Fe coordination motif facilitated O-O bond cleavage in O3.
• Achieved 100% ozonation efficiency for CH3SH elimination, outperforming MnO2 by 1,200-fold.

Conclusions:

• The Fe-Fe coordination in dinuclear sites enhances catalytic ozonation performance.
• Provides atomic-level insights into catalyst design for ozonation reactions.
• Demonstrates the potential of dinuclear catalysts beyond current applications.